Matuszak Daniel, Aranovich Gregory L, Donohue Marc D
Department of Chemical and Biomolecular Engineering, The Johns Hopkins University, Baltimore, Maryland 21218, USA.
J Chem Phys. 2004 Jul 1;121(1):426-35. doi: 10.1063/1.1756131.
A density functional theory of diffusion is developed for lattice fluids with molecular flux as a functional of the density distribution. The formalism coincides exactly with the generalized Ono-Kondo density functional theory when there is no gradient of chemical potential, i.e., at equilibrium. Away from equilibrium, it gives Fick's first law in the absence of a potential energy gradient, and it departs from Fickian behavior consistently with the Maxwell-Stefan formulation. The theory is applied to model a nanopore, predicting nonequilibrium phase transitions and the role of surface diffusion in the transport of capillary condensate.
针对晶格流体，发展了一种扩散的密度泛函理论，其中分子通量是密度分布的泛函。当不存在化学势梯度时，即处于平衡态时，该形式体系与广义小野 - 近藤密度泛函理论完全一致。在远离平衡态时，在不存在势能梯度的情况下，它给出菲克第一定律，并且它与麦克斯韦 - 斯蒂芬公式一致地偏离菲克行为。该理论被应用于对纳米孔进行建模，预测非平衡相变以及表面扩散在毛细管凝聚传输中的作用。
